We demonstrate one-dimensional Doppler cooling of a beam of buffer-gas cooled Barium monofluoride (BaF) molecules. The dependences of the cooling efficiency with the laser detuning, the bias filed and the laser intensity are carefully measured. We numerical simulate our experiment with a Monte Carlo method, and find the theoretic predictions consists with our experimental data. This result represents a key step towards further cooling and trapping of BaF molecules.
We theoretically investigate the laser cooling of fermionic barium monofluoride (137BaF) molecules, which are promising candidates for precision studies of weak parity violation and nuclear anapole moments. This molecular species features two nuclear spins, resulting in a hyperfine structure that is considerably more complicated than the one found in the usual laser-cooled diatomics. We use optical Bloch equations and rate equations to show that optical cycling, sub-Doppler cooling and bichromatic forces can all be realized under realistically achievable experimental conditions.
We demonstrate buffer-gas cooling, high-resolution spectroscopy and cycling fluorescence of cold barium monofluoride (BaF) molecules. Our source produces an intense and internally cold molecular beam containing the different BaF isotopologues with a mean forward velocity of 190 m/s. For a well-collimated beam of 138BaF we observe a flux of more than 1e10 molecules/sr/pulse in the X2Sigma, N=1 state in our downstream detection region. Studying the absorption line strength of the intermediate A'Delta state we infer a lifetime of 790+\-346 ns, significantly longer than previously estimated. Final…
We report an experimental investigation on the Doppler-free saturated absorption spectroscopy of buffer-gas-cooled Barium monofluoride (BaF) molecules in a 4~K cryogenic cell. The obtained spectra with a resolution of 19~MHz, much smaller than previously observed in absorption spectroscopy, clearly resolve the hyperfine transitions. Moreover, we use these high-resolution spectra to fit the hyperfine splittings of excited $A(v=0)$ state and find the hyperfine splitting of the laser-cooling-relevant $A^2Π_{1/2}(v=0, J=1/2, +)$ state is about 18 MHz, much higher than the previous theoretically pr…
A full density-matrix simulation is performed for optical deflection of a barium monofluoride (BaF) beam. Pairs of counter-propagating laser pulses are used for stimulated absorption followed by stimulated emission. The scheme produces a force which is nearly an order of magnitude larger than that obtainable using continuous-wave laser deflection, and yields a force-to-spontaneous-decay ratio which is more than an order of magnitude larger. The large reduction in spontaneous decay is key to optical deflection of molecules, where branching ratios to other vibrational states do not allow for cyc…
Calculations of the BaF-Ar triatomic system are performed with a relativistic Hamiltonian and coupled cluster theory at the CCSD(T) level for 1386 positions of the Ar atom relative to the BaF molecule. Calculations are repeated with increasing basis sets (double-, triple-, quadruple- and quintuple-zeta), and these are extrapolated to estimate the complete-basis-set limit. The resulting energies provide a potential energy for the interaction of an Ar atom with a BaF molecule. A fit is presented that parametrizes this potential. This work is needed for an understanding of the position, modes of …
Calculation of the local environment of a barium monofluoride molecule in an argon matrix: A step towards using matrix-isolated BaF for determining the electron electric dipole moment
本文计算了嵌入氩基质中 BaF 分子的局部环境，发现取代四个 Ar 原子最具优势，且低温下阻碍分子迁移与转动的势垒足以固定其位置和方向，为 EDM$^3$ 合作组精密测量电子电偶极矩提供了关键基础。
We have produced sympathetically cooled barium monohalide ions BaX$^+$ (X = F, Cl, Br) by reacting trapped, laser cooled Ba$^+$ ions with room temperature gas phase neutral halogen-containing molecules. Reaction rates for two of these (SF$_6$ and CH$_3$Cl) have been measured and are in agreement with classical models. BaX$^+$ ions are promising candidates for cooling to the rovibrational ground state, and our method presents a straightforward way to produce these polar molecular ions.
We study sympathetic cooling of the radial ion motion in a linear RF trap in mixed barium-ytterbium chains. Barium ions are Doppler-cooled, while ytterbium ions are cooled through their interaction with cold barium ions. We estimate the efficiency of sympathetic cooling by measuring the average occupation quantum numbers, and thus the temperature, of all radial normal modes of motion in the ion chain. The full set of orderings in a chain of two barium and two ytterbium ions have been probed, and we show that the average thermal occupation numbers for all chain configurations strongly depend on…
Gas-phase multiply charged proteins have been sympathetically cooled to translational temperatures below 1 K by Coulomb interaction with laser-cooled barium ions in a linear ion trap. In one case, an ensemble of 53 cytochrome c molecules (mass ~ 12390 amu, charge +17 e) was cooled by ~ 160 laser-cooled barium ions to less than 0.75 K. Storage times of more than 20 minutes have been observed and could easily be extended to more than an hour. The technique is applicable to a wide variety of complex molecules.
Calcium monofluoride (CaF) molecules are loaded into an optical dipole trap (ODT) and subsequently laser cooled within the trap. Starting with magneto-optical trapping, we sub-Doppler cool CaF and then load $150(30)$ CaF molecules into an ODT. Enhanced loading by a factor of five is obtained when sub-Doppler cooling light and trapping light are on simultaneously. For trapped molecules, we directly observe efficient sub-Doppler cooling to a temperature of $60(5)$ $μ\text{K}$. The trapped molecular density of $8(2)\times10^7$ cm$^{-3}$ is an order of magnitude greater than in the initial sub-Dop…
We reported a detailed experimental study of the cold collision of Barium monofluoride (BaF) with buffer gas and the high-resolution spectroscopy relevant with direct laser cooling. BaF molecules are efficiently produced with laser ablation and buffer-gas cooled in a cryogenic apparatus. The laser cooling relevant transition $|X^2Σ, v=0, N=1\rangle$ to $|A^2Π, v'=0, J'=1/2\rangle$ is identified. The collision cross section with buffer gas is measured to be $1.4(7)\times10^{-14} cm^{-2}$, which is very suitable for buffer gas cooling. Both rotational and vibrational temperatures are effectively…
First laser cooling and trapping of the heavy alkaline earth element barium has been achieved based on the strong 6s$^2$ $^1$S$_0$ - 6s6p $^1$P$_1$ transition for the main cooling. Due to the large branching into metastable D-states several additional laser driven transitions are required to provide a closed cooling cycle. A total efficiency of $0.4(1) \cdot 10^{-2}$ for slowing a thermal atomic beam and capturing atoms into a magneto optical trap was obtained. Trapping lifetimes of more than 1.5 s were observed. This lifetime is shortened at high laser intensities by photo ionization losses. …
Spectroscopic studies of aluminum monofluoride (AlF) have revealed its highly favorable properties for direct laser cooling. All $Q$ lines of the strong A$^1Π$ $\leftarrow$ X$^1Σ^+$ transition around 227~nm are rotationally closed and thereby suitable for the main cooling cycle. The same holds for the narrow, spin-forbidden a$^3Π$ $\leftarrow$ X$^1Σ^+$ transition around 367 nm which has a recoil limit in the micro Kelvin range. We here report on the spectroscopic characterization of the lowest rotational levels in the a$^3Π$ state of AlF for $v=0-8$ using a jet-cooled, pulsed molecular beam. A…
Barium monohydride (BaH) is an attractive candidate for extending laser cooling and trapping techniques to diatomic hydrides. The apparatus and high-resolution optical spectroscopy presented here demonstrate progress toward this goal. A cryogenic buffer-gas-cooled molecular beam of BaH was constructed and characterized. Pulsed laser ablation into cryogenic helium buffer gas delivers $\sim1\times10^{10}$ molecules/sr/pulse in the X$^2Σ^+$ ($v''=0,N''=1$) state of primary interest. More than $1\times10^7$ of these molecules per pulse enter the downstream science region with forward velocities be…
Efficient self-interference of single-photons emitted by a sideband-cooled Barium ion is demonstrated. First, the technical tools for performing efficient coupling to the quadrupolar transition of a single $^{138}$Ba$^{+}$ ion are presented. We show efficient Rabi oscillations of the internal state of the ion using a highly stabilized 1.76 $μm$ fiber laser resonant with the S$_{1/2}$-D$_{5/2}$ transition. We then show sideband cooling of the ion's motional modes and use it as a means to enhance the interference contrast of the ion with its mirror-image to up to 90%. Last, we measure the depend…
Specular reflection of polar molecules from a simple multi-cylinder electrostatic mirror: a method for separating BaF molecules produced in a buffer-gas-cooled laser-ablation source from other ablation products
We investigate the merits of a measurement of the permanent electric dipole moment of the electron ($e$EDM) with barium monofluoride molecules, thereby searching for phenomena of CP violation beyond those incorporated in the Standard Model of particle physics. Although the BaF molecule has a smaller enhancement factor in terms of the effective electric field than other molecules used in current studies (YbF, ThO and ThF$^+$), we show that a competitive measurement is possible by combining Stark-deceleration, laser-cooling and an intense primary cold source of BaF molecules. With the long coher…
We demonstrate a scheme for magneto-optically trapping strontium monofluoride (SrF) molecules at temperatures one order of magnitude lower and phase space densities three orders of magnitude higher than obtained previously with laser-cooled molecules. In our trap, optical dark states are destabilized by rapidly and synchronously reversing the trapping laser polarizations and the applied magnetic field gradient. The number of molecules and trap lifetime are also significantly improved from previous work by loading the trap with high laser power and then reducing the power for long-term trapping…
Cooling the rotation and the vibration of molecules by broadband light sources was possible for trapped molecular ions or ultracold molecules. Because of a low power spectral density, the cooling timescale has never fell below than a few milliseconds. Here we report on rotational and vibrational cooling of a supersonic beam of barium monofluoride molecules in less than 440 $μ$s. Vibrational cooling was optimized by enhancing the spectral power density of a semiconductor light source at the underlying molecular transitions allowing us to transfer all the populations of $v''=1-3$ into the vibrat…
Time resolved detection of laser induced fluorescence from pulsed excitation of electronic states in barium monofluoride (BaF) molecules has been performed in order to determine the lifetimes of the $A^2Π_{1/2}$ and $A^2Π_{3/2}$ states. The method permits control over experimental parameters such that systematic biases in the interpretation of the data can be controlled to below $10^{-3}$ relative accuracy. The statistically limited values for the lifetimes of the $A^2Π_{1/2}(ν=0)$ and $A^2Π_{3/2}(ν=0)$ states are 57.1(3) ns and 47.9(7)~ns, respectively. The ratio of these values is in good ag…
In this work, we demonstrate measurements of photodestruction rates of translationally cold, charged biomolecules. The long-term stable storage of the molecular ions in an ion trap at ultra-high vacuum conditions allows measurement of small rates and verification that rates are linear in photodestruction laser intensity. Measurements were performed on singly protonated molecules of the organic compound glycyrrhetinic acid (C30H46O4), dissociated by a continuous-wave UV laser (266 nm) using different intensities. The molecules were sympathetically cooled by simultaneously trapped laser-cooled b…
A cryogenic apparatus with a rotatable substrate for matrix isolation spectroscopy of BaF in neon crystals down to 3.2 K
Istituto Nazionale di Fisica Nucleare（意大利国家核物理研究所）；University of Ferrara（费拉拉大学）；University of Padua（帕多瓦大学）；National Quantum Science and Technology Institute（国家量子科学与技术研究所）
In order to realize more sensitive eEDM measurement, it would be worthwhile to find some new laser-cooled molecules with larger internal effective electric field (E$_{eff}$), higher electric polarizability and longer lifetime of the eEDM measurement state. Here we explore the merits of mercuric monofluoride ($^{202}Hg^{19}F$, X$^ 2 Σ_{1/2}$) for its potential of laser cooling and eEDM measurement. We theoretically investigated the electronic, rovibrational and hyperfine structures and verified the highly diagonal Franck-Condon factors (FCFs) of the main transitions by the Rydberg-Klein-Rees in…
Optically trapped laser-cooled polar molecules hold promise for new science and technology in quantum information and quantum simulation. Large numerical aperture optical access and long trap lifetimes are needed for many studies, but these requirements are challenging to achieve in a magneto-optical trap (MOT) vacuum chamber that is connected to a cryogenic buffer gas beam source, as is the case for all molecule laser cooling experiments so far. Long distance transport of molecules greatly eases fulfilling these requirements as molecules are placed into a region separate from the MOT chamber.…
Sympathetic cooling of trapped ions through collisions with neutral buffer gases is critical to a variety of modern scientific fields, including fundamental chemistry, mass spectrometry, nuclear and particle physics, and atomic and molecular physics. Despite its widespread use over four decades, there remain open questions regarding its fundamental limitations. To probe these limits, here we examine the steady-state evolution of up to ten barium ions immersed in a gas of three-million laser-cooled calcium atoms. We observe and explain the emergence of nonequilibrium behavior as evidenced by bi…
Production and spectroscopy of cold radioactive molecules
California Institute of Technology（加州理工学院）；Yale University（耶鲁大学）；Johns Hopkins University（约翰斯·霍普金斯大学）；Massachusetts Institute of Technology（麻省理工学院）；Michigan State University（密歇根州立大学）
It has been roughly three decades since laser cooling techniques produced ultracold atoms, leading to rapid advances in a vast array of fields. Unfortunately laser cooling has not yet been extended to molecules because of their complex internal structure. However, this complexity makes molecules potentially useful for many applications. For example, heteronuclear molecules possess permanent electric dipole moments which lead to long-range, tunable, anisotropic dipole-dipole interactions. The combination of the dipole-dipole interaction and the precise control over molecular degrees of freedom …
We study theoretically the behavior of laser-cooled calcium monofluoride (CaF) molecules in an optical molasses and magneto-optical trap (MOT), and compare our results to recent experiments. We use multi-level optical Bloch equations to estimate the force and the diffusion constant, followed by a Fokker-Planck-Kramers equation to calculate the time-evolution of the velocity distribution. The calculations are done in three-dimensions, and we include all the relevant energy levels of the molecule and all the relevant frequency components of the light. Similar to simpler model systems, the veloci…
Design and Performance of a Heated Gas Injector for Producing Cold Molecular Beams
Harvard/MIT Center for Ultracold Atoms（哈佛/麻省理工超冷原子中心）；Department of Physics, Harvard University（哈佛大学物理系）；Division of Engineering Science, University of Toronto（多伦多大学工程科学部）；Department of Physics, Massachusetts Institute of Technology（麻省理工学院物理系）
